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Surface species in CO and CO{sub 2} hydrogenation over copper/zirconia: On the methanol synthesis mechanism

Journal Article · · Langmuir
DOI:https://doi.org/10.1021/la9506990· OSTI ID:420714
 [1]; ;  [2];  [1]
  1. Paul Scherrer Institut, Villigen (Switzerland)
  2. ETH Zentrum, Zuerich (Switzerland)

Hydrogenation reactions occurring on the surface of a copper/zirconia (Cu:Zr = 30:70 atom %)catalyst, which had previously been loaded by adsorption of formic acid, CO, and CO{sub 2}, have been studied by means of in situ diffuse reflectance FTIR spectroscopy. Besides characterizing the reactivity of adsorbates, the dynamics of CO and CO{sub 2}/hydrogen reactant mixtures has been monitored over both the prereduced and unreduced catalyst, with the aim of acquiring information on the methanol synthesis mechanism. Surface formates, which have previously been identified as intermediates in the catalytic reduction of carbon oxides yielding methane, appear to be spectator species in methanol synthesis over ZrO{sub 2} supported catalysts. The latter synthesis, when using CO{sub 2} as the reactant, starts from surface carbonate, which is first reduced to yield adsorbed carbon monoxide and water. The desired methanol product is generated via surface-bound formaldehyde and methoxy species. 83 refs., 10 figs.

OSTI ID:
420714
Journal Information:
Langmuir, Journal Name: Langmuir Journal Issue: 22 Vol. 12; ISSN 0743-7463; ISSN LANGD5
Country of Publication:
United States
Language:
English